Volume holographic recording of information is an attractive solution for the next generation of digital storage systems, for the ability to optically record and retrieve, independently, multiple superimposed holograms, transferring in parallel the corresponding page-formated digital data representations. Due to these two unique properties, a holographic digital data storage (HDDS) system holds promise for high capacity density (Tb/cm 3 ), and fast transfer rate (Gb/sec) [1]. During holographic recording, information is stored as refractive index modulation, i.e. volume phase gratings, resulting from the interference of the information-bearing and reference laser beams within the volume of the holographic recording medium. The performance of a holographic storage system is principally determined by the physical characteristics of the recording medium [2]. Photorefractives have been the most extensively investigated materials utilized in holographic storage. Recently, advancements in sufficiently thick photopolymer holographic media have provided a promising alternative for WORM systems [3, 4]. In these materials, formation of compositional volume phase gratings through a photoinitiated polymerization process provides an attractive recording mechanism which allows for relatively large permanent refractive index modulation with high recording sensitivity, that compares favorably to, typically volatile, recording in photorefractives [4, 5, 6]. Limitations in the response of these materials, however, may arise during and after exposure, limiting the sensitivity, the final grating strength, and the digital system performance. In this presentation, we evaluate the physical properties that allow for efficient volume holographic recording utilizing photoinitiated polymerization grating formation. The previous studies of photoinitiated polymerization recording, in materials utilizing a free-radical [4], or a cationing-ring-opening (crop) [7] process, have suggested limited grating strength to arise due to reciprocity failure at high intensity, and at large grating spacing recordings. Grating formation has further been described through a photoinduced reaction diffusion model that ignores postexposure polymerization (dark reaction), and introduces diffusion limited response for multiple recordings [4]. In this presentation, we evaluate photopolymer recording in a unified framework based on the polymerization (τ p ) and the diffusion (τ d = Λ 2 /D) time scales that completely characterize the principal physical processes during grating formation [8]. We investigated elaborately holographic recording in a material utilizing cationing-ring-opening polymerization (crop Polaroid samples).